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On healable polymers and fiber-reinforced composites

Abstract

Polymeric materials capable of healing damage would be valuable in structural applications where access for repair is limited. Approaches to creating such materials are reviewed, with the present work focusing on polymers with thermally reversible covalent cross-links. These special cross-links are Diels-Alder (DA) adducts, which can be separated and re-formed, enabling healing of mechanical damage at the molecular level. Several DA-based polymers, including 2MEP4FS, are mechanically and thermally characterized. The polymerization reaction of 2MEP4FS is modeled and the number of established DA adducts is associated with the glass transition temperature of the polymer. The models are applied to concentric cylinder rotational measurements of 2MEP4FS prepolymer at room and elevated temperatures to describe the viscosity as a function of time, temperature, and conversion. Mechanical damage including cracks and scratches are imparted in cured polymer samples and subsequently healed. Damage due to high temperature thermal degradation is observed to not be reversible. The ability to repair damage without flowing polymer chains makes DA-based healable polymers particularly well-suited for crack healing. The double cleavage drilled compression (DCDC) fracture test is investigated as a useful method of creating and incrementally growing cracks in a sample. The effect of sample geometry on the fracture behavior is experimentally and computationally studied. Computational and empirical models are developed to estimate critical stress intensity factors from DCDC results. Glass and carbon fiber-reinforced composites are fabricated with 2MEP4FS as the matrix material. A prepreg process is developed that uses temperature to control the polymerization rate of the monomers and produce homogeneous prepolymer for integration with a layer of unidirectional fiber. Multiple prepreg layers are laminated to form multi-layered cross-ply healable composites, which are characterized in bending using dynamic mechanical analysis (DMA). Simple, theory-based analyses indicate that numerous cracks are present before testing due to thermal expansion mismatches, and during testing, these cracks must be healing. Extending healable composites to include healable fiber-matrix interfaces is discussed as future work and interfacial healing characterization approaches are considered

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